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Global monitoring of aerosols is required to analyse the impacts of aerosols on air quality and to understand their role in modulating the climate variability. The Copernicus Atmosphere Monitoring Service (CAMS) provides near real time forecasts and reanalyses of aerosols using the ECMWF Integrated Forecasting System (IFS), constrained by the assimilation of MODIS and PMAp Aerosol Optical Depth (AOD). Given the potential end-of-lifetime of MODIS AOD, implementing new AOD observations in the CAMS operational suite is a priority to ensure the continuity of the CAMS forecast performances. The objective of this work is to test the assimilation of the NOAA VIIRS AOD product from S-NPP and NOAA20 satellites in the IFS model. Simulation experiments assimilating VIIRS on top or in place of MODIS were carried out from June 2021 to November 2021 to evaluate the impacts on the AOD analysis. For maritime aerosol background, the assimilation of VIIRS and the use of VIIRS from NOAA20 as an anchor reduce the analysis AOD values compared to MODIS-based experiments, in which the analysis values were too high due to the positive bias of MODIS/TERRA over ocean. Over land, the assimilation of VIIRS induces a large increase in the analysis over biomass burning regions where VIIRS shows larger AOD than MODIS. For dust source regions, the analysis is reduced when VIIRS is assimilated on top of or in place of MODIS, particularly over the Sahara, Arabian Peninsula and few places in Asia in the July-August period. The assimilation of VIIRS leads to an overall reduction of the bias in AOD analysis evaluated against AERONET measurements with the largest bias reduction over Europe, desert, and maritime sites.

The Copernicus Atmosphere Monitoring Service (CAMS) has recently produced a greenhouse gas reanalysis (version egg4) that covers almost 2 decades from 2003 to 2020 and which will be extended in the future. This reanalysis dataset includes carbon dioxide (CO2) and methane (CH4). The reanalysis procedure combines model data with satellite data into a globally complete and consistent dataset using the European Centre for Medium-Range Weather Forecasts' Integrated Forecasting System (IFS). This dataset has been carefully evaluated against independent observations to ensure validity and to point out deficiencies to the user. The greenhouse gas reanalysis can be used to examine the impact of atmospheric greenhouse gas concentrations on climate change (such as global and regional climate radiative forcing), assess intercontinental transport, and serve as boundary conditions for regional simulations, among other applications and scientific uses. The caveats associated with changes in assimilated observations and fixed underlying emissions are highlighted, as is their impact on the estimation of trends and annual growth rates of these long-lived greenhouse gases.

Tropopause folds are the key process underlying stratosphere-to-troposphere transport (STT) of ozone, and thus they affect tropospheric ozone levels and variability. In the present study we perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 during folding events over Europe and for the time period from 2003 to 2018. A 3-D labeling algorithm is applied to detect tropopause folds in CAMSRA, while ozonesonde data from WOUDC (World Ozone and Ultraviolet Radiation Data Centre) and aircraft measurements from IAGOS (In-service Aircraft for a Global Observing System) are used for CAMSRA O3 evaluation. The profiles of observed and CAMSRA O3 concentrations indicate that CAMSRA reproduces the observed O3 increases in the troposphere during the examined folding events. Nevertheless, at most of the examined sites, CAMSRA overestimates the observed O3 concentrations, mostly at the upper portion of the observed increases, with a median fractional gross error (FGE) among the examined sites >0.2 above 400 hPa. The use of a control run without data assimilation reveals that the aforementioned overestimation of CAMSRA O3 arises from the data assimilation implementation. Overall, although data assimilation assists CAMSRA O3 to follow the observed O3 enhancements in the troposphere during the STT events, it introduces biases in the upper troposphere resulting in no clear quantitative improvement compared to the control run without data assimilation. Less biased assimilated O3 products, with finer vertical resolution in the troposphere, in addition to higher IFS (Integrated Forecasting System) vertical resolution, are expected to provide a better representation of O3 variability during tropopause folds.

The Copernicus Atmosphere Monitoring Service (CAMS) operated by the European Centre for Medium-Range Weather Forecasts (ECMWF) has produced a global reanalysis of aerosol and reactive gases (called CAMSRA) for the period 2003–2016. Space observations of ozone, carbon monoxide, NO2 and aerosol optical depth are assimilated by a 4D-Var method in the 60-layer ECMWF global atmospheric model, which for the reanalysis is operated at a horizontal resolution of about 80 km. As a contribution to the evaluation of the reanalysis, we compare atmospheric concentrations of different reactive species provided by the CAMS reanalysis with independent observational data gathered by airborne instrumentation during the field campaigns INTEX-A, INTEX-B, NEAQS-ITCT, ITOP, AMMA, ARCTAS, VOCALS, YAK-AEROSIB, HIPPO and KORUS-AQ. We show that the reanalysis rather successfully reproduces the observed concentrations of chemical species that are assimilated in the system, including O3 and CO with biases generally less than 20 %, but generally underestimates the concentrations of the primary hydrocarbons and secondary organic species. In some cases, large discrepancies also exist for fast-reacting radicals such as OH and HO2.

The Copernicus Atmosphere Monitoring Service (CAMS), operated by the European Centre for Medium-Range Weather Forecasts on behalf of the European Commission, provides daily analyses and 5 d forecasts of atmospheric composition, including forecasts of volcanic sulfur dioxide (SO2) in near real time. CAMS currently assimilates total column SO2 products from the GOME-2 instruments on MetOp-B and MetOp-C and the TROPOMI instrument on Sentinel-5P, which give information about the location and strength of volcanic plumes. However, the operational TROPOMI and GOME-2 data do not provide any information about the height of the volcanic plumes, and therefore some prior assumptions need to be made in the CAMS data assimilation system about where to place the resulting SO2 increments in the vertical. In the current operational CAMS configuration, the SO2 increments are placed in the mid-troposphere, around 550 hPa or 5 km. While this gives good results for the majority of volcanic emissions, it will clearly be wrong for eruptions that inject SO2 at very different altitudes, in particular exceptional events where part of the SO2 plume reaches the stratosphere. A new algorithm, developed by the German Aerospace Centre (DLR) for GOME-2 and TROPOMI, optimized in the frame of the ESA-funded Sentinel-5P Innovation–SO2 Layer Height Project, and known as the Full-Physics Inverse Learning Machine (FP_ILM) algorithm, retrieves SO2 layer height from TROPOMI in near real time (NRT) in addition to the SO2 column. CAMS is testing the assimilation of these products, making use of the NRT layer height information to place the SO2 increments at a retrieved altitude. Assimilation tests with the TROPOMI SO2 layer height data for the Raikoke eruption in June 2019 show that the resulting CAMS SO2 plume heights agree better with IASI plume height data than operational CAMS runs without the TROPOMI SO2 layer height information and show that making use of the additional layer height information leads to improved SO2 forecasts. Including the layer height information leads to higher modelled total column SO2 values in better agreement with the satellite observations. However, the plume area and SO2 burden are generally also overestimated in the CAMS analysis when layer height data are used. The main reason for this overestimation is the coarse horizontal resolution used in the minimizations. By assimilating the SO2 layer height data, the CAMS system can predict the overall location of the Raikoke SO2 plume up to 5 d in advance for about 20 d after the initial eruption, which is better than with the operational CAMS configuration (without prior knowledge of the plume height) where the forecast skill is much more reduced for longer forecast lead times.

Concentrations of atmospheric methane (CH4), the second most important greenhouse gas, continue to grow. In recent years this growth rate has increased further (2020: +14.7 ppb), the cause of which remains largely unknown. Here, we demonstrate a high-resolution (~80 km), short-window (24-hour) 4D-Var global inversion system based on the ECMWF Integrated Forecasting System (IFS) and newly available satellite observations. The largest national disagreement found between prior (63.1 Tg yr−1) and posterior (59.8 Tg yr−1) CH4 emissions is from China, mainly attributed to the energy sector. Emissions estimated form our global system agree well with previous basin-wide regional studies and point source specific studies. Emission events (leaks/blowouts) >10 t hr−1 were detected, but without accurate prior uncertainty information, were not well quantified. Our results suggest that global anthropogenic CH4 emissions for 2020 were 5.7 Tg yr−1 (+1.6 %) higher than for 2019, mainly attributed to the energy and agricultural sectors. Regionally, the largest 2020 increases were seen from China (+2.6 Tg yr−1, 4.3 %), with smaller increases from India (+0.8 Tg yr−1, 2.2 %) and Indonesia (+0.3 Tg yr−1, 2.6 %). Results show the rise in emissions, and subsequent atmospheric growth, would have occurred with or without the COVID-19 slowdown. During the onset of the global slowdown (March–April, 2020) energy sector CH4 emissions from China increased; however, during later months (May–June, 2020) emissions decreased below expected pre-slowdown levels. The accumulated impact of the slowdown on CH4 emissions from March–June 2020 is found to be small. Changes in atmospheric chemistry, not investigated here, may have contributed to the observed growth in 2020. Future work aims to develop the global IFS inversion system and to extend the 4D-Var window-length using a hybrid ensemble-variational method.

The Copernicus Atmosphere Monitoring Service (CAMS) reanalysis is the latest global reanalysis dataset of atmospheric composition produced by the European Centre for Medium-Range Weather Forecasts (ECMWF), consisting of three-dimensional time-consistent atmospheric composition fields, including aerosols and chemical species. The dataset currently covers the period 2003–2016 and will be extended in the future by adding 1 year each year. A reanalysis for greenhouse gases is being produced separately. The CAMS reanalysis builds on the experience gained during the production of the earlier Monitoring Atmospheric Composition and Climate (MACC) reanalysis and CAMS interim reanalysis. Satellite retrievals of total column CO; tropospheric column NO2; aerosol optical depth (AOD); and total column, partial column and profile ozone retrievals were assimilated for the CAMS reanalysis with ECMWF's Integrated Forecasting System. The new reanalysis has an increased horizontal resolution of about 80 km and provides more chemical species at a better temporal resolution (3-hourly analysis fields, 3-hourly forecast fields and hourly surface forecast fields) than the previously produced CAMS interim reanalysis. The CAMS reanalysis has smaller biases compared with most of the independent ozone, carbon monoxide, nitrogen dioxide and aerosol optical depth observations used for validation in this paper than the previous two reanalyses and is much improved and more consistent in time, especially compared to the MACC reanalysis. The CAMS reanalysis is a dataset that can be used to compute climatologies, study trends, evaluate models, benchmark other reanalyses or serve as boundary conditions for regional models for past periods.

Global tropospheric ozone reanalyses constructed using different state-of-the-art satellite data assimilation systems, prepared as part of the Copernicus Atmosphere Monitoring Service (CAMS-iRean and CAMS-Rean) as well as two fully independent reanalyses (TCR-1 and TCR-2, Tropospheric Chemistry Reanalysis), have been intercompared and evaluated for the past decade. The updated reanalyses (CAMS-Rean and TCR-2) generally show substantially improved agreements with independent ground and ozone-sonde observations over their predecessor versions (CAMS-iRean and TCR-1) for diurnal, synoptical, seasonal, and interannual variabilities. For instance, for the Northern Hemisphere (NH) mid-latitudes the tropospheric ozone columns (surface to 300 hPa) from the updated reanalyses show mean biases to within 0.8 DU (Dobson units, 3 % relative to the observed column) with respect to the ozone-sonde observations. The improved performance can likely be attributed to a mixture of various upgrades, such as revisions in the chemical data assimilation, including the assimilated measurements, and the forecast model performance. The updated chemical reanalyses agree well with each other for most cases, which highlights the usefulness of the current chemical reanalyses in a variety of studies. Meanwhile, significant temporal changes in the reanalysis quality in all the systems can be attributed to discontinuities in the observing systems. To improve the temporal consistency, a careful assessment of changes in the assimilation configuration, such as a detailed assessment of biases between various retrieval products, is needed. Our comparison suggests that improving the observational constraints, including the continued development of satellite observing systems, together with the optimization of model parameterizations such as deposition and chemical reactions, will lead to increasingly consistent long-term reanalyses in the future.

The TROPOspheric Monitoring Instrument (TROPOMI) on board the Sentinel 5 Precursor (S5P) satellite launched in October 2017 yields a wealth of atmospheric composition data, including retrievals of total column ozone (TCO3) that are provided in near-real time (NRT) and off-line. These NRT TCO3 retrievals (V1.0.0) have been included in the data assimilation system of the Copernicus Atmosphere Monitoring Service (CAMS), and tests to monitor the data and to carry out first assimilation experiments with them have been performed for the period 26 November 2017 to 3 May 2018. TROPOMI was still in its commissioning phase until 24 April 2018. Nevertheless, the results show that, even at this early stage, the TROPOMI TCO3 data generally agree well with the CAMS analysis over large parts of the Globe and also with TCO3 retrievals from the Ozone Monitoring Instrument (OMI) and the Global Ozone Monitoring Experiment-2 (GOME-2) that are routinely assimilated by CAMS. However, the TCO3 NRT data from TROPOMI show some retrieval anomalies at high latitudes, at low solar elevations and over snow/ice (e.g. Antarctica) where the differences with the CAMS analysis and the other datasets are larger. These differences come mainly from the surface albedo climatology that is used in the NRT TROPOMI TCO3 retrieval. This climatology has a coarser horizontal resolution than the TROPOMI TCO3 data which leads to problems in areas where there are large changes in reflectivity from pixel to pixel, e.g. pixels covered by snow/ice or not. The assimilation of TROPOMI TCO3 has been tested in the CAMS system for data between 60°N and 60°S and for solar elevations less than 10° and is found to have only little impact on the ozone analysis, because the CAMS analysis is already well constrained by several other ozone retrievals that are routinely assimilated. Variational bias correction is applied to the TROPOMI NRT TCO3 data and successfully corrects for the biases seen in the data. Averaged over the period 26 November 2017 to 3 May 2018, difference between experiments with and without assimilation of TROPOMI data are less than 2% for TCO3 and less than 1% in the vertical for averaged zonal mean O3 mixing ratios. Compared to independent observation (Brewer spectrometers, ozone sondes, IAGOS ozone profiles and GAW surface measurements) the differences between the assimilation run and a run without TROPOMI assimilation are also small. The only noteworthy differences between the experiment with and without assimilation of TROPOMI data are seen compared to IAGOS profiles at West African airports where the assimilation of TROPOMI improves the fit of the CAMS analysis to the independent data. Despite the small impact of TROPOMI TCO3 in the CAMS analysis it will be beneficial to include the TROPOMI TCO3 NRT data actively in the operational NRT CAMS analysis after more tests. This will add some redundancy and resilience in the system and will allow us to use a more robust observation system in case some of the other older instruments, whose retrievals are currently assimilated by CAMS, stop working.

Stratosphere-to-troposphere transport (STT) is an important natural source of tropospheric ozone, which can occasionally influence ground-level ozone concentrations relevant for air quality. Here, we analyse and evaluate the Copernicus Atmosphere Monitoring Service (CAMS) global and regional forecast systems during a deep STT event over Europe for the time period from 4 to 9 January 2017. The predominant synoptic condition is described by a deep upper level trough over eastern and central Europe, favouring the formation of tropopause folding events along the jet stream axis and therefore the intrusion of stratospheric ozone into the troposphere. Both global and regional CAMS forecast products reproduce the “hook-shaped” streamer of ozone-rich and dry air in the middle troposphere depicted from the observed satellite images of water vapour. The CAMS global model successfully reproduces the folding of the tropopause at various European sites, such as Trapani (Italy), where a deep folding down to 550 hPa is seen. The stratospheric ozone intrusions into the troposphere observed by WOUDC ozonesonde and IAGOS aircraft measurements are satisfactorily forecasted up to 3 days in advance by the CAMS global model in terms of both temporal and vertical features of ozone. The fractional gross error (FGE) of CAMS ozone day 1 forecast between 300 and 500 hPa is 0.13 over Prague, while over Frankfurt it is 0.04 and 0.19, highlighting the contribution of data assimilation, which in most cases improves the model performance. Finally, the meteorological and chemical forcing of CAMS global forecast system in the CAMS regional forecast systems is found to be beneficial for predicting the enhanced ozone concentrations in the middle troposphere during a deep STT event.

This work is an extended evaluation of near-surface ozone as part of the global reanalysis of atmospheric composition, produced within the European-funded project MACC (Monitoring Atmospheric Composition and Climate). It includes an evaluation over the period 2003–2012 and provides an overall assessment of the modeling system performance with respect to near-surface ozone for specific European subregions. Measurements at rural locations from the European Monitoring and Evaluation Program (EMEP) and the European Air Quality Database (AirBase) were used for the evaluation assessment. The fractional gross error of near-surface ozone reanalysis is on average 24 % over Europe, the highest found over Scandinavia (27 %) and the lowest over the Mediterranean marine stations (21 %). Near-surface ozone shows mostly a negative bias in winter and a positive bias during warm months. Assimilation reduces the bias in near-surface ozone in most of the European subregions – with the exception of Britain and Ireland and the Iberian Peninsula and its impact is mostly notable in winter. With respect to the seasonal cycle, the MACC reanalysis reproduces the photochemically driven broad spring-summer maximum of surface ozone of central and south Europe. However, it does not capture adequately the early spring peak and the shape of the seasonality at northern and north-eastern Europe. The diurnal range of surface ozone, which is as an indication of the local photochemical production processes, is reproduced fairly well, with a tendency for a small overestimation during the warm months for most subregions (especially in central and southern Europe). Possible reasons leading to discrepancies between the MACC reanalysis and observations are discussed.

The El Niño–Southern Oscillation (ENSO) not only affects meteorological fields but also has a large impact on atmospheric composition. Atmospheric composition fields from the Monitoring Atmospheric Composition and Climate (MACC) reanalysis are used to identify the ENSO signal in tropospheric ozone, carbon monoxide, nitrogen oxide and smoke aerosols, concentrating on the months October to December. During El Niño years, all of these fields have increased concentrations over maritime South East Asia in October. The MACC Composition Integrated Forecasting System (C-IFS) model is used to quantify the relative magnitude of dynamically induced and emission-driven changes in the atmospheric composition fields. While changes in tropospheric ozone are a combination of dynamically induced and emission-driven changes, the changes in carbon monoxide, nitrogen oxides and smoke aerosols are almost entirely emission-driven in the MACC model. The ozone changes continue into December, i.e. after the end of the Indonesian fire season while changes in the other fields are confined to the fire season.

A new global reanalysis data set of atmospheric composition (AC) for the period 2003–2015 has been produced by the Copernicus Atmosphere Monitoring Service (CAMS). Satellite observations of total column (TC) carbon monoxide (CO) and aerosol optical depth (AOD), as well as several TC and profile observations of ozone, have been assimilated with the Integrated Forecasting System for Composition (C-IFS) of the European Centre for Medium-Range Weather Forecasting. Compared to the previous Monitoring Atmospheric Composition and Climate (MACC) reanalysis (MACCRA), the new CAMS interim reanalysis (CAMSiRA) is of a coarser horizontal resolution of about 110 km, compared to 80 km, but covers a longer period with the intent to be continued to present day. This paper compares CAMSiRA with MACCRA and a control run experiment (CR) without assimilation of AC retrievals. CAMSiRA has smaller biases than the CR with respect to independent observations of CO, AOD and stratospheric ozone. However, ozone at the surface could not be improved by the assimilation because of the strong impact of surface processes such as dry deposition and titration with nitrogen monoxide (NO), which were both unchanged by the assimilation. The assimilation of AOD led to a global reduction of sea salt and desert dust as well as an exaggerated increase in sulfate. Compared to MACCRA, CAMSiRA had smaller biases for AOD, surface CO and TC ozone as well as for upper stratospheric and tropospheric ozone. Finally, the temporal consistency of CAMSiRA was better than the one of MACCRA. This was achieved by using a revised emission data set as well as by applying careful selection and bias correction to the assimilated retrievals. CAMSiRA is therefore better suited than MACCRA for the study of interannual variability, as demonstrated for trends in surface CO.

This paper demonstrates that SO2 columnar amounts have significantly increased following the five largest volcanic eruptions of the past decade in the Northern Hemisphere. A strong positive signal was detected by all the existing networks either ground based (Brewer, EARLINET, AirBase) or from satellites (OMI, GOME-2). The study particularly examines the adequacy of the existing Brewer network to detect SO2 plumes of volcanic origin in comparison to other networks and satellite platforms. The comparison with OMI and GOME-2 SO2 space-borne retrievals shows statistically significant agreement between the Brewer network data and the collocated satellite overpasses. It is shown that the Brewer instrument is capable of detecting significant columnar SO2 increases following large volcanic eruptions, when SO2 levels rise well above the instrumental noise of daily observations, estimated to be of the order of 2 DU. A model exercise from the MACC project shows that the large increases of SO2 over Europe following the Bárðarbunga eruption in Iceland were not caused by local sources or ship emissions but are clearly linked to the eruption. We propose that by combining Brewer data with that from other networks and satellites, a useful tool aided by trajectory analyses and modeling could be created which can be used to forecast high SO2 values both at ground level and in air flight corridors following future eruptions.

In September and October 2015 widespread forest and peatland fires burned over large parts of maritime southeast Asia, most notably Indonesia, releasing large amounts of terrestrially-stored carbon into the atmosphere, primarily in the form of CO2, CO and CH4. With a mean emission rate of 11.3 Tg CO2 per day during Sept-Oct 2015, emissions from these fires exceeded the fossil fuel CO2 release rate of the European Union (EU28) (8.9 Tg CO2 per day). Although seasonal fires are a frequent occurrence in the human modified landscapes found in Indonesia, the extent of the 2015 fires was greatly inflated by an extended drought period associated with a strong El Niño. We estimate carbon emissions from the 2015 fires to be the largest seen in maritime southeast Asia since those associated with the record breaking El Niño of 1997. Compared to that event, a much better constrained regional total carbon emission estimate can be made for the 2015 fires through the use of present-day satellite observations of the fire’s radiative power output and atmospheric CO concentrations, processed using the modelling and assimilation framework of the Copernicus Atmosphere Monitoring Service (CAMS) and combined with unique in situ smoke measurements made on Kalimantan.

Carbon monoxide (CO) is a key atmospheric compound that can be remotely sensed by satellite on the global scale. Fifteen years of continuous observations are now available from the MOPITT/Terra mission (2000 to present). Another 15 and more years of observations will be provided by the IASI/MetOp instrument series (2007-2023 >). In order to study long-term variability and trends, a homogeneous record is required, which is not straightforward as the retrieved quantities are instrument and processing dependent. The present study aims at evaluating the consistency between the CO products derived from the MOPITT and IASI missions, both for total columns and vertical profiles, during a 6-year overlap period (2008-2013). The analysis is performed by first comparing the available 2013 versions of the retrieval algorithms (v5T for MOPITT and v20100815 for IASI), and second using a dedicated reprocessing of MOPITT CO profiles and columns using the same a priori information as the IASI product. MOPITT total columns are generally slightly higher over land (bias ranging from 0 to 13 %) than IASI data. When IASI and MOPITT data are retrieved with the same a priori constraints, correlation coefficients are slightly improved. Large discrepancies (total column bias over 15 %) observed in the Northern Hemisphere during the winter months are reduced by a factor of 2 to 2.5. The detailed analysis of retrieved vertical profiles compared with collocated aircraft data from the MOZAIC-IAGOS network, illustrates the advantages and disadvantages of a constant vs. a variable a priori. On one hand, MOPITT agrees better with the aircraft profiles for observations with persisting high levels of CO throughout the year due to pollution or seasonal fire activity (because the climatology-based a priori is supposed to be closer to the real atmospheric state). On the other hand, IASI performs better when unexpected events leading to high levels of CO occur, due to a larger variability associated with the a priori., SCOPUS: ar.j, info:eu-repo/semantics/published

Daily global analyses and 5-day forecasts are generated in the context of the European Monitoring Atmospheric Composition and Climate (MACC) project using an extended version of the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The IFS now includes modules for chemistry, deposition and emission of reactive gases, aerosols, and greenhouse gases, and the 4-dimensional variational data assimilation scheme makes use of multiple satellite observations of atmospheric composition in addition to meteorological observations. This paper describes the data assimilation setup of the new Composition-IFS (C-IFS) with respect to reactive gases and validates analysis fields of ozone (O3), carbon monoxide (CO), and nitrogen dioxide (NO2) for the year 2008 against independent observations and a control run without data assimilation. The largest improvement in CO by assimilation of Measurements of Pollution in the Troposphere (MOPITT) CO columns is seen in the lower troposphere of the Northern Hemisphere (NH) extratropics during winter, and during the South African biomass-burning season. The assimilation of several O3 total column and stratospheric profile retrievals greatly improves the total column, stratospheric and upper tropospheric O3 analysis fields relative to the control run. The impact on lower tropospheric ozone, which comes from the residual of the total column and stratospheric profile O3 data, is smaller, but nevertheless there is some improvement particularly in the NH during winter and spring. The impact of the assimilation of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI) is small because of the short lifetime of NO2, suggesting that NO2 observations would be better used to adjust emissions instead of initial conditions. The results further indicate that the quality of the tropospheric analyses and of the stratospheric ozone analysis obtained with the C-IFS system has improved compared to the previous "coupled" model system of MACC.

A representation of atmospheric chemistry has been included in the Integrated Forecasting System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The new chemistry modules complement the aerosol modules of the IFS for atmospheric composition, which is named C-IFS. C-IFS for chemistry supersedes a coupled system in which chemical transport model (CTM) Model for OZone and Related chemical Tracers 3 was two-way coupled to the IFS (IFS-MOZART). This paper contains a description of the new on-line implementation, an evaluation with observations and a comparison of the performance of C-IFS with MOZART and with a re-analysis of atmospheric composition produced by IFS-MOZART within the Monitoring Atmospheric Composition and Climate (MACC) project. The chemical mechanism of C-IFS is an extended version of the Carbon Bond 2005 (CB05) chemical mechanism as implemented in CTM Transport Model 5 (TM5). CB05 describes tropospheric chemistry with 54 species and 126 reactions. Wet deposition and lightning nitrogen monoxide (NO) emissions are modelled in C-IFS using the detailed input of the IFS physics package. A 1 year simulation by C-IFS, MOZART and the MACC re-analysis is evaluated against ozonesondes, carbon monoxide (CO) aircraft profiles, European surface observations of ozone (O3), CO, sulfur dioxide (SO2) and nitrogen dioxide (NO2) as well as satellite retrievals of CO, tropospheric NO2 and formaldehyde. Anthropogenic emissions from the MACC/CityZen (MACCity) inventory and biomass burning emissions from the Global Fire Assimilation System (GFAS) data set were used in the simulations by both C-IFS and MOZART. C-IFS (CB05) showed an improved performance with respect to MOZART for CO, upper tropospheric O3, and wintertime SO2, and was of a similar accuracy for other evaluated species. C-IFS (CB05) is about 10 times more computationally efficient than IFS-MOZART.

The Monitoring Atmospheric Composition and Climate (MACC) project represents the European Union's Copernicus Atmosphere Monitoring Service (CAMS) (http://www.copernicus.eu/), which became fully operational during 2015. The global near-real-time MACC model production run for aerosol and reactive gases provides daily analyses and 5-day forecasts of atmospheric composition fields. It is the only assimilation system worldwide that is operational to produce global analyses and forecasts of reactive gases and aerosol fields. We have investigated the ability of the MACC analysis system to simulate tropospheric concentrations of reactive gases covering the period between 2009 and 2012. A validation was performed based on carbon monoxide (CO), nitrogen dioxide (NO2) and ozone (O3) surface observations from the Global Atmosphere Watch (GAW) network, the O3 surface observations from the European Monitoring and Evaluation Programme (EMEP) and, furthermore, NO2 tropospheric columns, as well as CO total columns, derived from satellite sensors. The MACC system proved capable of reproducing reactive gas concentrations with consistent quality; however, with a seasonally dependent bias compared to surface and satellite observations – for northern hemispheric surface O3 mixing ratios, positive biases appear during the warm seasons and negative biases during the cold parts of the year, with monthly modified normalised mean biases (MNMBs) ranging between −30 and 30 % at the surface. Model biases are likely to result from difficulties in the simulation of vertical mixing at night and deficiencies in the model's dry deposition parameterisation. Observed tropospheric columns of NO2 and CO could be reproduced correctly during the warm seasons, but are mostly underestimated by the model during the cold seasons, when anthropogenic emissions are at their highest level, especially over the US, Europe and Asia. Monthly MNMBs of the satellite data evaluation range from values between −110 and 40 % for NO2 and at most −20 % for CO, over the investigated regions. The underestimation is likely to result from a combination of errors concerning the dry deposition parameterisation and certain limitations in the current emission inventories, together with an insufficiently established seasonality in the emissions.

In this study we compare the diurnal variation in stratospheric ozone derived from free-running simulations of the Whole Atmosphere Community Climate Model (WACCM) and from reanalysis data of the atmospheric service MACC (Monitoring Atmospheric Composition and Climate) which both use a similar stratospheric chemistry module. We find good agreement between WACCM and the MACC reanalysis for the diurnal ozone variation in the high-latitude summer stratosphere based on photochemistry. In addition, we consult the ozone data product of the ERA-Interim reanalysis. The ERA-Interim reanalysis ozone system with its long-term ozone parametrization can not capture these diurnal variations in the upper stratosphere that are due to photochemistry. The good dynamics representations, however, reflects well dynamically induced ozone variations in the lower stratosphere. For the high-latitude winter stratosphere we describe a novel feature of diurnal variation in ozone where changes of up to 46.6% (3.3 ppmv) occur in monthly mean data. For this effect good agreement between the ERA-Interim reanalysis and the MACC reanalysis suggest quite similar diurnal advection processes of ozone. The free-running WACCM model seriously underestimates the role of diurnal advection processes at the polar vortex at the two tested resolutions. The intercomparison of the MACC reanalysis and the ERA-Interim reanalysis demonstrates how global reanalyses can benefit from a chemical representation held by a chemical transport model. The MACC reanalysis provides an unprecedented description of the dynamics and photochemistry of the diurnal variation of stratospheric ozone which is of high interest for ozone trend analysis and research on atmospheric tides. We confirm the diurnal variation in ozone at 5 hPa by observations of the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) experiment and selected sites of the Network for Detection of Atmospheric Composition Change (NDACC). The latter give valuable insight even to diurnal variation of ozone in the polar winter stratosphere.

An eight-year long reanalysis of atmospheric composition data covering the period 2003-2010 was constructed as part of the FP7-funded Monitoring Atmospheric Composition and Climate project by assimilating satellite data into a global model and data assimilation system. This reanalysis provides fields of chemically reactive gases, namely carbon monoxide, ozone, nitrogen oxides, and formaldehyde, as well as aerosols and greenhouse gases globally at a horizontal resolution of about 80 km for both the troposphere and the stratosphere. This paper describes the assimilation system for the reactive gases and presents validation results for the reactive gas analysis fields to document the data set and to give a first indication of its quality. Tropospheric CO values from the MACC reanalysis are on average 10-20% lower than routine observations from commercial aircrafts over airports through most of the troposphere, and have larger negative biases in the boundary layer at urban sites affected by air pollution, possibly due to an underestimation of CO or precursor emissions. Stratospheric ozone fields from the MACC reanalysis agree with ozonesondes and ACE-FTS data to within ±10% in most seasons and regions. In the troposphere the reanalysis shows biases of -5% to +10% with respect to ozonesondes and aircraft data in the extratropics, but has larger negative biases in the tropics. Area-averaged total column ozone agrees with ozone fields from a multi-sensor reanalysis data set to within a few percent. NO2 fields from the reanalysis show the right seasonality over polluted urban areas of the NH and over tropical biomass burning areas, but underestimate wintertime NO2 maxima over anthropogenic pollution regions and overestimate NO2 in northern and southern Africa during the tropical biomass burning seasons. Tropospheric HCHO is well simulated in the MACC reanalysis even though no satellite data are assimilated. It shows good agreement with independent SCIAMACHY retrievals over regions dominated by biogenic emissions with some anthropogenic input, such as the eastern US and China, and also over African regions influenced by biogenic sources and biomass burning. © Author(s) 2013., SCOPUS: re.j, info:eu-repo/semantics/published

The severe wildfires in western Russia during July–August 2010 coincided with a strong heat wave and led to large emissions of aerosols and trace gases such as carbon monoxide (CO), hydrocarbons and nitrogen oxides into the troposphere. This extreme event is used to evaluate the ability of the global MACC (Monitoring Atmospheric Composition and Climate) atmospheric composition forecasting system to provide analyses of large-scale pollution episodes and to test the respective influence of a priori emission information and data assimilation on the results. Daily 4-day hindcasts were conducted using assimilated aerosol optical depth (AOD), CO, nitrogen dioxide (NO2) and ozone (O3) data from a range of satellite instruments. Daily fire emissions were used from the Global Fire Assimilation System (GFAS) version 1.0, derived from satellite fire radiative power retrievals. The impact of accurate wildfire emissions is dominant on the composition in the boundary layer, whereas the assimilation system influences concentrations throughout the troposphere, reflecting the vertical sensitivity of the satellite instruments. The application of the daily fire emissions reduces the area-average mean bias by 63% (for CO), 60% (O3) and 75% (NO2) during the first 24 h with respect to independent satellite observations, compared to a reference simulation with a multi-annual mean climatology of biomass burning emissions. When initial tracer concentrations are further constrained by data assimilation, biases are reduced by 87, 67 and 90%. The forecast accuracy, quantified by the mean bias up to 96 h lead time, was best for all compounds when using both the GFAS emissions and assimilation. The model simulations suggest an indirect positive impact of O3 and CO assimilation on hindcasts of NO2 via changes in the oxidizing capacity. However, the quality of local hindcasts was strongly dependent on the assumptions made for forecasted fire emissions. This was well visible from a relatively poor forecast accuracy quantified by the root mean square error, as well as the temporal correlation with respect to ground-based CO total column data and AOD. This calls for a more advanced method to forecast fire emissions than the currently adopted persistency approach. The combined analysis of fire radiative power observations, multiple trace gas and aerosol satellite observations, as provided by the MACC system, results in a detailed quantitative description of the impact of major fires on atmospheric composition, and demonstrate the capabilities for the real-time analysis and forecasts of large-scale fire events.

The 2008 Antarctic ozone hole was one of the largest and most long-lived in recent years. Predictions of the ozone hole were made in near-real time (NRT) and hindcast mode with the Integrated Forecast System (IFS) of the European Centre for Medium-Range Weather Forecasts (ECMWF). The forecasts were carried out both with and without assimilation of satellite observations from multiple instruments to provide more realistic initial conditions. Three different chemistry schemes were applied for the description of stratospheric ozone chemistry: (i) a linearization of the ozone chemistry, (ii) the stratospheric chemical mechanism of the MOZART-3 chemical transport model (CTM) and (iii) the relaxation to a climatology as implemented in the TM5 CTM. The IFS uses the latter two schemes by means of a two-way coupled system. Without assimilation, the forecasts showed model-specific shortcomings in predicting start time, extent and duration of the ozone hole. The assimilation of satellite observations from the Microwave Limb Sounder (MLS), the Ozone Monitoring Instrument (OMI), the Solar Backscattering Ultraviolet radiometer (SBUV-2) and the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY) led to a significant improvement of the forecasts when compared with total columns and vertical profiles from ozone sondes. The combined assimilation of observations from multiple instruments helped to overcome limitations of the ultraviolet (UV) sensors at low solar elevation over Antarctica. The assimilation of data from MLS was crucial to obtain a good agreement with the observed ozone profiles both in the polar stratosphere and troposphere. The ozone analyses by the three model configurations were very similar despite the different underlying chemistry schemes. During the chemically instigated development of the ozone hole, differences quickly developed in the initialized forecasts by the different schemes. The predictions of the ozone-hole closure, which is driven mainly by dynamical processes, benefited from the initialization over a much longer forecast length. The characteristics of the individual chemistry schemes became apparent after the third forecast day but the forecasts were still close to the respective analyses. The initialization with ozone analyses was beneficial up to at least 15 days.

Vertical profiles of CO taken from the MOZAIC aircraft database are used to globally evaluate the performance of the GEMS/MACC models, including the ECMWF-Integrated Forecasting System (IFS) model coupled to the CTM MOZART-3 with 4DVAR data assimilation for the year 2004. This study provides a unique opportunity to compare the performance of three offline CTMs (MOZART-3, MOCAGE and TM5) driven by the same meteorology as well as one coupled atmosphere/CTM model run with data assimilation, enabling us to assess the potential gain brought by the combination of online transport and the 4DVAR chemical satellite data assimilation. First we present a global analysis of observed CO seasonal averages and interannual variability for the years 2002–2007. Results show that despite the intense boreal forest fires that occurred during the summer in Alaska and Canada, the year 2004 had comparably lower tropospheric CO concentrations. Next we present a validation of CO estimates produced by the MACC models for 2004, including an assessment of their ability to transport pollutants originating from the Alaskan/Canadian wildfires. In general, all the models tend to underestimate CO. The coupled model and the CTMs perform best in Europe and the US where biases range from 0 to -25% in the free troposphere and from 0 to -50% in the surface and boundary layers (BL). Using the 4DVAR technique to assimilate MOPITT V4 CO significantly reduces biases by up to 50% in most regions. However none of the models, even the IFS-MOZART-3 coupled model with assimilation, are able to reproduce well the CO plumes originating from the Alaskan/Canadian wildfires at downwind locations in the eastern US and Europe. Sensitivity tests reveal that deficiencies in the fire emissions inventory and injection height play a role.

The implementation and application of a newly developed coupled system combining ECMWF's integrated forecast system (IFS) with global chemical transport models (CTMs) is presented. The main objective of the coupled system is to enable the IFS to simulate key chemical species without the necessity to invert the complex source and sink processes such as chemical reactions, emission and deposition. Thus satellite observations of atmospheric composition can be assimilated into the IFS using its 4D-VAR algorithm. In the coupled system, the IFS simulates only the transport of chemical species. The coupled CTM provides to the IFS the concentration tendencies due to emission injection, deposition and chemical conversion. The CTMs maintain their own transport schemes and are fed with meteorological data at hourly resolution from the IFS. The CTM used in the coupled system can be either MOZART-3, TM5 or MOCAGE. The coupling is achieved via the special-purpose OASIS4 software. The scientific integrity of the coupled system is proven by analysing the difference between stand-alone CTM simulations and the tracer fields in the coupled IFS. The IFS concentration fields match the CTM fields for about 48 h with the biggest differences occurring in the planetary boundary layer (PBL). The coupled system is a good test bed for process-oriented comparison of the coupled CTM. As an example, the vertical structure of chemical conversion and emission injection is studied for a ten day period over Central Europe for the three CTMs.

This study provides a comprehensive assessment of NO2 changes across the main European urban areas induced by the COVID-19 lockdown using satellite retrievals from the Tropospheric Monitoring Instrument (TROPOMI), surface site measurements and simulations from the Copernicus Atmospheric Monitoring Service (CAMS) regional ensemble of air quality models. Some recent TROPOMI-based estimates of NO2 changes have neglected the influence of weather variability between the reference and lockdown periods. Here we provide weather-normalized estimates based on a machine learning method (gradient boosting) along with an assessment of the biases that can be expected from methods that omit the influence of weather. We also compare the weather-normalized satellite NO2 column changes with both weather-normalized surface NO2 concentration changes and simulated changes by the CAMS regional ensemble, composed of 11 models, using recently published emission reductions induced by the lockdown. We show that all estimates show the same tendency on NO2 reductions. Locations where the lockdown was stricter show stronger reductions and, conversely, locations where softer measures were implemented show milder reductions in NO2 pollution levels. Regarding average reductions, estimates based on either satellite observations (−23 %) surface stations (−43 %) or models (−32 %) are presented, showing the importance of vertical sampling but also the horizontal representativeness. Surface station estimates are significantly changed when sampled to the TROPOMI overpasses (−37 %) pointing out the importance of the variability in time of such estimates. Observation based machine learning estimates show a stronger temporal variability than the model-based estimates.